Carbon dioxide reduction catalyzed by dinuclear ruthenium polypyridyl complexes

Takashi Ono, Nora Planas, Pere Mirõ, Mehmed Z. Ertem, Eduardo C. Escudero-Adán, Jordi Benet-Buchholz, Laura Gagliardi, Christopher J. Cramer, Antoni Llobet

Research output: Contribution to journalArticleResearchpeer-review

7 Citations (Scopus)

Abstract

Dinuclear ruthenium complexes [(Ru(bid)) 2 (μ-bpp)(μ-OAc)] and [(Ru(trpy)) 2 (μ-bpp)(μ-X)] 2+ [X=Cl - , OAc - , and OCHO - ; bpp=3,5-bis(2-pyridyl)pyrazolato; bid - =(1Z,3Z)-1,3-bis(pyridin-2-ylmethylene)isoindolin-2-ide; trpy=2,2':6',2"-terpyridine] were tested as catalysts for the hydrogenative reduction of carbon dioxide in the solvent 2,2,2-trifluoroethanol in the presence of excess amine (triethylamine). Significant amounts of formic acid were produced by these catalysts, and a kinetic analysis based on initial rate constants was performed. These catalytic systems were investigated by using DFT calculations to elucidate the hydrogenative reduction mechanism. The results are compared with those obtained with previously reported mononuclear catalyst counterparts. Carbon footprints: New dinuclear ruthenium complexes that act as efficient catalysts for the hydrogenative reduction of carbon dioxide to formic acid have been prepared and fully characterized. The kinetics associated with the catalytic cycle were studied experimentally and a full catalytic cycle was determined on the basis of DFT calculations, which complement the experimental results. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Original languageEnglish
Pages (from-to)3897-3903
JournalChemCatChem
Volume5
Issue number12
DOIs
Publication statusPublished - 1 Dec 2013

Keywords

  • carbon dioxide reduction
  • density functional calculations
  • dinuclear complexes
  • polypyridyl
  • ruthenium

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